Abstract: Coffee grounds are promising precursors for excellent porous carbon adsorbents. During the preparation of the porous carbons, sodium silicate was used as a binder and pore-forming agent, and extrusion molding technology was used to prepare them in a columnar form. After carbonization, steam activation and silica removal by alkaline washing, high-strength columnar porous carbon adsorbents (CGCs) were obtained. Their CH₄/N₂ separation performance was studied by multicomponent breakthrough experiments. The Brunauer-Emmett-Teller (BET) surface area of CGC-1.5 (where 1.5 is the mass ratio of a 9 wt% sodium silicate aqueous solution to the coffee grounds) is 527 m²·g⁻¹. Both the N₂ and CO₂ adsorption isotherms show that the CGCs are rich in micropores and mesopores, with the micropores mainly centered at about 0.48 nm. FT-IR results show that CGC-1.5 has abundant oxygen-containing functional groups. At 298 K and 1 bar, its equilibrium adsorption capacity for CH₄ is 0.87 mmol·g⁻¹, and the separation selectivity for a CH₄/N₂ mixture (3/7, vol/vol) is 10.3, which is better than most biomass-based porous carbon adsorbents and crystalline materials. Dynamic breakthrough tests show that CGC-1.5 has an excellent CH₄/N₂ separation performance at both high and atmospheric pressures. The dynamic selectivities at 298 K, 1.1 bar and 5 bar are 10.4 and 17.9, respectively. The adsorption capacity is unchanged after 10 adsorption-desorption cycles. The mechanical strength of CGC-1.5 is as high as 123 N·cm⁻¹, which meets the criteria of industrial applications.